首页|K-CuZnZrO2系列催化剂的制备及其对CO加氢合成低碳醇性能的影响

K-CuZnZrO2系列催化剂的制备及其对CO加氢合成低碳醇性能的影响

扫码查看
通过共沉淀-浸渍法制备了一系列K-CuZnZrO2催化剂,研究了 Cu质量分数对合成气(CO+H2)制低碳醇(异丁醇)的影响.在该系列K-CuZnZrO2催化剂上,低碳醇中甲醇和异丁醇是主要产物(总醇收率达95%).Cu质量分数为12%的K-12%CuZnZrO2催化剂表现出最优的异丁醇合成性能,异丁醇选择性为20.2%,异丁醇收率为22.8 g/(L.h).综合多种表征分析结果表明:改变Cu质量分数可以实现对Cu-Zr相互作用的调控.Cu和无定形ZrO2之间的电子转移,能够显著促进Cu2+还原的同时产生低强度的弱碱位点,特别是利于产生更多高分散的CuO-ZrO2固溶体,这对CO加氢协同催化形成异丁醇至关重要.过量的Cu组分将破坏CuO-ZrO2固溶体的电子和配位结构,Cu-Zr之间相互作用减弱,抑制C-C链的增长,降低异丁醇选择性.研究结果将为进一步定向调控设计高效、高选择性、高稳定性异丁醇合成催化剂提供新思路.
Preparation of K-CuZnZrO2 Series Catalysts and Their Effect on the Performance of CO Hydrogenation for Low-Carbon Alcohol Synthesis
A series of K-CuZnZrO2 catalysts were synthesized using co-precipitation and impregnation methods to investigate the influence of Cu content on the production of lower alcohols,specifically isobutanol,from syngas(CO+H2).Among the products obtained using the K-CuZnZrO2 catalysts,methanol and isobutanol were the pri-mary products(comprising 95%of the total alcohols).The K-12%CuZnZrO2 catalyst with the Cu mass fraction of 12%demonstrated the highest performance for isobutanol synthesis,with an isobutanol selectivity of 20.2%and a yield of 22.8 g/(L-h).Various characterization analyses indicated that altering the Cu component effectively regu-lates the Cu-Zr interaction.Electron transfer between Cu and amorphous ZrO2 significantly promotes the reduction of Cu2+while generating low-strength weak alkaline sites,which favor the formation of more highly dispersed CuO-ZrO2 solid solutions.These solid solutions are critical for the synergistic catalytic synthesis of isobutanol via CO hy-drogenation.An excess of Cu content disrupts the electronic and coordination structure of the CuO-ZrO2 solid solu-tion,weakens the Cu-Zr interaction,inhibits the growth of C-C chains,and ultimately reduces isobutanol selec-tivity.The results provide new perspectives for the design of efficient,highly selective,and stable catalysts for isobutanol synthesis.

CO hydrogenationsynergistic catalysislower alcoholsCuO-ZrO2 solid solution

杨佳茜、金嘉钰、薛凯凯、李旭达、郭腾罄、汪钰熠、卫晨飞、薛朵梅、智丽飞、孙凯

展开 >

太原科技大学化学工程与技术学院,太原 030024

山西医科大学第一附属医院,太原 030001

CO加氢 协同催化 低碳醇 CuO-ZrO2 固溶体

2024

华南师范大学学报(自然科学版)
华南师范大学

华南师范大学学报(自然科学版)

CSTPCD北大核心
影响因子:0.413
ISSN:1000-5463
年,卷(期):2024.56(5)